Boosting Hot Electron-Driven Photocatalysis through Anisotropic Plasmonic Nanoparticles with Hot Spots in Au-TiO2 Nanoarchitectures
Boosting Hot Electron-Driven Photocatalysis through Anisotropic Plasmonic Nanoparticles with Hot Spots in Au-TiO2 Nanoarchitectures
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DOI：
10.1021/acs.jpcc.6b02370
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发表时间：
2016-06-02
影响因子：
3.7
通讯作者：
Correa-Duarte, Miguel A.
中科院分区：
文献类型：
--
作者：
Sousa-Castillo, Ana;Comesana-Hermo, Miguel;Correa-Duarte, Miguel A.
等离子体金属纳米粒子作为光敏剂的使用在过去几年中得到了强劲的发展，因为它们能够增加半导体的活性，进入可见光和近红外区。本文报道了金纳米颗粒形状各向异性对金-二氧化钛纳米结构光催化性能影响的实验和理论研究。研究结果表明，对于一定数量的金属材料，与Au纳米球或纳米棒的存在相比，Au纳米星赋予了二氧化钛极强的催化效率。这归因于纳米恒星在其尖峰周围局部产生极大的电磁场增强的能力，这确保了在金属和半导体之间的界面附近增加热电子的数量。因此，这些纳米结构呈现出一种可以被描述为等离子体热点光催化的新颖的光催化活性区域。数值模拟证实了热电子注入是光敏化过程背后的一种可行的机制，并且纳米星应该具有最强的光化学响应。这些结果为在可见光和近红外下工作的高性能光催化纳米反应的等离子体组分的合理设计铺平了道路。
The use of plasmonic metal nanoparticles as photo sensitizers has undergone a strong development in the past few years given their ability-to-increase the activity of,semiconductors into the visible and near-infrared regions. The present work reports an experimental and theoretical study on the critical influence that shape anisotropy of gold nanoparticles exerts on the photocatalytic performance of Au-TiO2 nanoarchitectures. The obtained results show that for a given amount of metallic material, Au nanostars endow titania with a strongly enhanced catalytic,efficiency,compared to that found in the presence of Au nanospheres or nanorods. This is ascribed to the ability of nanostars to locally create extremely-large, electromagnetic field enhancements around their spikes, which ensures an increased population of hot electrons close to the interface between the metal and the semiconductor. Therefore, these nanostructures exhibit a, novel "regime of photocatalytic activity that could be described as plasmonic hot-spot photocatalysis. Numerical simulations confirm that the hot electron injection is a feasible Mechanism behind the photosensitization process and that the nanostars should have the strongest photochemical response. These results pave the way for a more rational design of the plasmonic component in the search for high-performance photocatalytic-nanoreactots operating under visible and NIR light.